We experimentally investigated the crystallographic anisotropy of the intrinsic Gilbert damping constant in single crystalline Fe(001) film deposited on MgO(001) substrate. The frequency-domain ferromagnetic resonance (FMR) spectrum was measured at given external magnetic fields via a vector network analyzer. From the field-domain FMR linewidth obtained as a function of resonant frequency, the intrinsic Gilbert damping constants along the crystallographic axes in the (001) plane were successfully obtained by evaluating the extrinsic influence of two magnon scattering and inhomogeneity. A four-fold crystalline anisotropy of the intrinsic Gilbert damping constant, similar to the magnetic crystalline anisotropy in the (001) plane, was clearly observed. Furthermore, we found that the intrinsic Gilbert damping constant along the easy axis was smaller than that along the hard axis.